In this study, a novel and exceedingly simple method for the aqueous synthesis of stable, unagglomerated polypyrrole nanospheres was investigated. The method is template- and surfactant-free and uses only pyrrole monomer, water, and ozone. When the monomer concentration, exposure time to ozone, and temperature were varied, it was determined that the temperature was the critical factor controlling the particle size through particle size measurements via dynamic light scattering and transmission electron microscopy (TEM). From the particle size measurements, a particle size distribution with a number-weighted mean diameter of 73 nm and a standard deviation of 18 nm was achieved. The particles were also investigated using λ-potential measurements, ultraviolet-visible (UV-vis) spectroscopy, Fourier transform infrared (FTIR) spectroscopy, and thermogravimetric analysis in an effort to determine the identity of the nanoparticles as well as the mechanism by which the nanoparticles are formed and stabilized.